The main objective is to determine compositional structural details of the inorganic phase in teeth and bones. Infrared and Raman spectroscopy as well as chemical methods are employed in these studies. Methods are devised for the preparation of synthetic calcium apatites having controlled physical properties (crystal size and perfection) and chemical constituents (e.g., hydroxide, fluoride, chloride, carbonate, water and acid phosphate). The vibrational spectra of these apatites and related compounds are assigned and characterized. Isotopically enriched apatite analogs are prepared to facilitate spectral assignments. The spectroscopic assignments and supplemental spectral data (temperature dependency and polarization) are then utilized to establish compositional and structural details of the apatites in question including: the type and geometry of constitutent ions; the site and number of sites occupied by the ions; orientation of ions; chemical bonding and interactions of ions; and semi-quantitative estimations of the constituents present. The results of findings for these controlled apatite systems are then related to the inorganic phase in calcified tissues.